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In this work, scattering mechanisms in the highly efficient thermoelectric material La_(3−x)Te_4 are investigated by controlling the carrier concentration via anion substitution in the nominally vacancy-free compositions La_3Te_(4−z)Sb_z and La_3Te_(4−z)Bi_z. Through a comparison of the lattice thermal conductivity κ_L in samples with and without Sb/Bi, this work reveals that La vacancies scatter phonons very efficiently and provide a ~100% reduction in κ_L at 575 K. The addition of Sb or Bi leads to a significant reduction in the band gap, which is observed in the temperature-dependent transport data as well as first-principles calculations. Despite this significant change to the band structure, the transport parameters of the conduction band are only slightly modified. Also, an increase in the Hall mobility is observed at high T and ...

Thermoelectric materials can be optimized by tuning the carrier concentration with chemical doping. However, because the optimum dopant concentration typically increases with temperature, the optimum efficiency can not normally be achieved for a uniform material in a temperature gradient. Here, we show Ag-doped PbTe/Ag_2Te composites exhibit high thermoelectric performance (∼50% greater than La-doped composites) because of a temperature induced gradient in the doping concentration caused by the temperature-dependent solubility of Ag in the PbTe matrix. This demonstrates a new mechanism to achieve a higher thermoelectric efficiency afforded by a given material system, and should be applicable to other thermoelectric materials.

Polycrystalline samples of LaRuAsO, NdRuAsO, SmRuAsO, and GdRuAsO have been
synthesized and studied using powder x-ray diffraction, electrical transport,
magnetization, and heat capacity measurements. Variations in structural
properties across the series reveal a trend toward more ideal tetrahedral
coordination around Ru as the size of the rare earth element is reduced. The
lattice parameters of these Ru compounds show a more anisotropic response to
variation in Ln than their Fe analogues, and significant anisotropy in thermal
expansion is also observed. Transport measurements show metallic behavior, and
carrier concentrations near 10^21 - 10^22 electrons per cm^3 are inferred from
simple analysis of Hall effect measurements. Anomalies in resistivity,
magnetization, and heat capacity indicate antiferromagnetic ordering of rare
earth ...

We investigate the carrier density and temperature dependence of the Seebeck coefficient of La_(3−x)Te_4 via
density-functional calculations and Boltzmann transport theory. The pertinent band structure has light bands at
the band gap and heavy degenerate bands with band minima near energies corresponding to the experimentally
determined optimum carrier density. Heavy bands increase the energy dependence of the density of states,
which increases the magnitude of the Seebeck coefficient in an itinerant conduction regime, while the light
bands provide a conduction channel that works against carrier localization promoted by La vacancies. The net
result is thermoelectric performance greater than current n-type materials above 1000 K.

Transport properties of the layered Zintl compound SrZnSb_2 have been characterized from room temperature to 725 K on polycrystalline samples. SrZnSb_2 samples were found to be p-type with a Hall carrier concentration of 5×10^(20) cm^(−3) at room temperature, and a small Seebeck coefficient and electrical resistivity are observed. A single band model predicts that, even with optimal doping, significant thermoelectric performance will not be achieved in SrZnSb_2. A relatively low lattice thermal conductivity is observed, κ_L~1.2 W m^(−1) K^(−1), at room temperature. The thermal transport of SrZnSb_2 is compared to that of the layered Zintl compounds AZn2Sb_2 (A=Ca,Yb,Sr,Eu), which have smaller unit cells and larger lattice thermal conductivity, κ_L~2 W m^(−1) K^(−1), at 300K. Ultrasonic measurements, in combination with kinetic theory a...

A low temperature, solid state synthesis technique has enabled the production of homogeneous samples of La_(3−x−y)Yb_yTe_4. This allows the substitution of divalent Yb to be utilized to optimize the thermoelectric performance in lanthanum telluride. The addition of Yb^(2+) changes the electrical transport properties in a manner that can be well understood using valence counting rules and a corresponding change in the Fermi energy. The substitution of Yb^(2+) for La^(3+) results in a threefold finer control over the carrier density n, thus allowing the optimum n ~ 0.3 × 10^(21) cm^(−3) to be both predicted and prepared. The net result is an improvement in thermoelectric efficiency, with zT reaching ~ 1.2 at 1273 K.

Zintl phases and related compounds are promising thermoelectric materials; for instance, high zT has been found in Yb_(14)MnSb_(11), clathrates, and the filled skutterudites. The rich solid-state chemistry of Zintl phases enables numerous possibilities for chemical substitutions and structural modifications that allow the fundamental transport parameters (carrier concentration, mobility, effective mass, and lattice thermal conductivity) to be modified for improved thermoelectric performance. For example, free carrier concentration is determined by the valence imbalance using Zintl chemistry, thereby enabling the rational optimization of zT. The low thermal conductivity values obtained in Zintl thermoelectrics arise from a diverse range of sources, including point defect scattering and the low velocity of optical phonon modes. Despite t...

The effects of various transition metal dopants on the electrical and thermal
transport properties of Fe1-xMxSi alloys (M= Co, Ir, Os) are reported. The
maximum thermoelectric figure of merit ZTmax is improved from 0.007 at 60 K for
pure FeSi to ZT = 0.08 at 100 K for 4% Ir doping. A comparison of the thermal
conductivity data among Os, Ir and Co doped alloys indicates strong
electron-phonon coupling in this compound. Because of this interaction, the
common approximation of dividing the total thermal conductivity into
independent electronic and lattice components ({\kappa}Total =
{\kappa}electronic + {\kappa}lattice) fails for these alloys. The effects of
grain size on thermoelectric properties of Fe0.96Ir0.04Si alloys are also
reported. The thermal conductivity can be lowered by about 50% with little or
no effect on the electrical r...

The thermoelectric transport properties of polycrystalline, Ba_(8)Ga_(16−x)Ge_(30+x) were characterized from 300 to 1000 K. The carrier density was found to vary precisely with the experimental x as expected from simple electron counting. The experimental data are analyzed within the framework of a single parabolic band model, which is found to accurately describe transport for the compositions of interest for thermoelectric application. The lattice thermal conductivity, calculated with a degeneracy adjusted Lorenz number, does not show a trend with composition and a value of ~1 Wm^(−1) K^(−1) is observed at 300 K. A maximum figure of merit zT = 0.86 is obtained at 950 K, and the optimal doping level for thermoelectric application is predicted to be ~2 × 10^(20) cm^(−3), which corresponds to Ba_(8)Ga_(15.75)Ge_(30.25_ by electron coun...

Comment: Copyright (2012) American Institute of Physics. This article may be
downloaded for personal use only. Any other use requires prior permission of
the author and the American Institute of Physics. The following article
appeared in (J. Appl. Phys. 111, 033708 (2012)) and may be found at
http://link.aip.org/link/?JAP/111/033708

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